U.S. Department of EnergyOffice of Scientific and Technical Information
Understanding the Origins of Higher Capacities at Faster Rates in Lithium-Excess LixNi2–4x/3Sbx/3O2
Abstract
Here, the lithium-excess LixNi2-4x/3Sbx/3O2 (LNSO) materials were previously shown to demonstrate higher capacities and improved cyclability with increasing lithium content. While the performance trend is promising, observed capacities are much lower than theoretical capacities, pointing to a need for further understanding of active redox processes in these materials. In this work, we study the electrochemical behavior of the LNSO materials as a function of lithium content and at slow and fast rates. Surprisingly, Li1.15Ni0.47Sb0.38O2 (LNSO-15) exhibits higher discharge capacities at faster rates and traverses distinct voltage curves at slow and fast rates. To understand these two peculiarities, we characterize the redox activity of nickel, antimony, and oxygen at different rates. While experiments confirm some nickel redox activity and oxygen loss, these two mechanisms cannot account for all observed capacity. We propose that the balance of the observed capacity may be due reversible oxygen redox and that the rate-dependent voltage curve features may derive from irreversible nickel migration occurring on slow charge. As future high energy density cathodes are likely to contain both lithium excess and high nickel content, both of these findings have important implications for the development of novel high capacity cathode materials.
- Authors:
-
[1];
- Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
- Technische Univ. Munchen, Garching (Germany)
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Paul Scherrer Inst. (PSI), Villigen (Switzerland)
- Harvard Univ., Cambridge, MA (United States)
- Georgia Inst. of Technology, Atlanta, GA (United States)
- Univ. of California, Berkeley, CA (United States)
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
- OSTI Identifier:
- 1476471
- Alternate Identifier(s):
- OSTI ID: 1374886
- Grant/Contract Number:
- AC02-05CH11231; AC02-06CH11357
- Resource Type:
- Journal Article: Accepted Manuscript
- Journal Name:
- Chemistry of Materials
- Additional Journal Information:
- Journal Volume: 29; Journal Issue: 6; Related Information: © 2017 American Chemical Society.; Journal ID: ISSN 0897-4756
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Twu, Nancy, Metzger, Michael, Balasubramanian, Mahalingam, Marino, Cyril, Li, Xin, Chen, Hailong, Gasteiger, Hubert, and Ceder, Gerbrand. Understanding the Origins of Higher Capacities at Faster Rates in Lithium-Excess LixNi2–4x/3Sbx/3O2. United States: N. p., 2017.
Web. doi:10.1021/acs.chemmater.6b04691.
Twu, Nancy, Metzger, Michael, Balasubramanian, Mahalingam, Marino, Cyril, Li, Xin, Chen, Hailong, Gasteiger, Hubert, & Ceder, Gerbrand. Understanding the Origins of Higher Capacities at Faster Rates in Lithium-Excess LixNi2–4x/3Sbx/3O2. United States. https://doi.org/10.1021/acs.chemmater.6b04691
Twu, Nancy, Metzger, Michael, Balasubramanian, Mahalingam, Marino, Cyril, Li, Xin, Chen, Hailong, Gasteiger, Hubert, and Ceder, Gerbrand. 2017.
"Understanding the Origins of Higher Capacities at Faster Rates in Lithium-Excess LixNi2–4x/3Sbx/3O2". United States. https://doi.org/10.1021/acs.chemmater.6b04691. https://www.osti.gov/servlets/purl/1476471.
@article{osti_1476471,
title = {Understanding the Origins of Higher Capacities at Faster Rates in Lithium-Excess LixNi2–4x/3Sbx/3O2},
author = {Twu, Nancy and Metzger, Michael and Balasubramanian, Mahalingam and Marino, Cyril and Li, Xin and Chen, Hailong and Gasteiger, Hubert and Ceder, Gerbrand},
abstractNote = {Here, the lithium-excess LixNi2-4x/3Sbx/3O2 (LNSO) materials were previously shown to demonstrate higher capacities and improved cyclability with increasing lithium content. While the performance trend is promising, observed capacities are much lower than theoretical capacities, pointing to a need for further understanding of active redox processes in these materials. In this work, we study the electrochemical behavior of the LNSO materials as a function of lithium content and at slow and fast rates. Surprisingly, Li1.15Ni0.47Sb0.38O2 (LNSO-15) exhibits higher discharge capacities at faster rates and traverses distinct voltage curves at slow and fast rates. To understand these two peculiarities, we characterize the redox activity of nickel, antimony, and oxygen at different rates. While experiments confirm some nickel redox activity and oxygen loss, these two mechanisms cannot account for all observed capacity. We propose that the balance of the observed capacity may be due reversible oxygen redox and that the rate-dependent voltage curve features may derive from irreversible nickel migration occurring on slow charge. As future high energy density cathodes are likely to contain both lithium excess and high nickel content, both of these findings have important implications for the development of novel high capacity cathode materials.},
doi = {10.1021/acs.chemmater.6b04691},
url = {https://www.osti.gov/biblio/1476471},
journal = {Chemistry of Materials},
issn = {0897-4756},
number = 6,
volume = 29,
place = {United States},
year = {Wed Feb 08 00:00:00 EST 2017},
month = {Wed Feb 08 00:00:00 EST 2017}
}
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